Engineering ion-pumping solid electrolyte interphase for ultra-stable aqueous zinc-ion batteries under deep discharge conditions

Abstract

Meeting the global terawatt-scale energy demands necessitates innovative solutions to overcome the critical challenges facing aqueous Zn-ion batteries, particularly the poor reversibility and unstable plating/stripping of Zn anodes under high depths of discharge (DOD). In this work, we introduce a novel composite artificial solid-electrolyte interphase (SEI), termed P-G, which combines a poly(ether-block-amide) matrix with graphene oxide (GO). By leveraging the functional groups of the polymer (C=O, C–O–C) and the electronegativity of GO, the P-G SEI layer acts as a highly efficient Zn2+ ion pump, achieving a remarkable Zn2+ transfer number of 0.77 and fast ion transport kinetics. Comprehensive theoretical and experimental analyses demonstrate that the P-G SEI layer regulates Zn2+ coordination and forms rapid ion transport pathways, leading to a highly stable and reversible Zn anode. As a result, P-G@Zn symmetric cells achieve ultra-stable cycling for 6500 hours at 1 mA·cm-2 and a record-breaking lifespan exceeding 5000 hours at 54.7% DOD. Furthermore, a high-specific-energy P-G@Zn||I2 pouch cell delivers exceptional performance, retaining 82.8% capacity after 400 cycles with an N/P ratio of 2. This study offers a compelling framework for designing advanced composite SEI layer, paving the way for highly reversible Zn-ion batteries in practical energy storage applications.

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Article information

Article type
Paper
Submitted
11 Mar 2025
Accepted
25 Jul 2025
First published
26 Jul 2025
This article is Open Access
Creative Commons BY-NC license

Energy Environ. Sci., 2025, Accepted Manuscript

Engineering ion-pumping solid electrolyte interphase for ultra-stable aqueous zinc-ion batteries under deep discharge conditions

L. Yang, Y. Shen, X. Long, Q. Ma, Z. Ruan, N. Xu, K. Li, L. Jiao, Y. Kong, J. Li, L. Tang, A. Yu and B. Cheng, Energy Environ. Sci., 2025, Accepted Manuscript , DOI: 10.1039/D5EE01408E

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